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At least 1,171 records · Page 65

High-Precision Mapping of Diamond Crystal Strain Using Quantum Interferometry

Crystal-strain variation imposes significant limitations on many quantum sensing and information applications for solid-state defect qubits in diamond. Thus, the precision measurement and control of diamond crystal strain is a key challenge. Here, we report diamond strain measurements with a unique set of capabilities, including micron-scale spatial resolution, a millimeter-scale field of view, and a 2-order-of-magnitude improvement in volume-normalized sensitivity over previous work, reaching 5(2)×10 -8 /√Hzμm -3 (with spin-strain coupling coefficients representing the dominant systematic uncertainty). We use strain-sensitive spin-state interferometry on ensembles of nitrogen-vacancy (N-V) color centers in single-crystal bulk diamond with low strain gradients. This quantum interferometry technique provides insensitivity to magnetic-field inhomogeneity from the electronic and nuclear spin bath, thereby enabling long N-V–ensemble electronic spin dephasing times and enhanced strain sensitivity, as well as broadening the potential applications of the technique beyond isotopically enriched or high-purity diamond. We demonstrate the strain-sensitive measurement protocol first on a confocal scanning laser microscope, providing quantitative measurement of sensitivity as well as three-dimensional strain mapping; and second on a wide-field-imaging quantum diamond microscope. Our strain-microscopy technique enables fast, sensitive characterization for diamond material engineering and nanofabrication; as well as diamond-based sensing of strains applied externally, as in diamond anvil cells or embedded diamond stress sensors, or internally, as by crystal damage due to particle-induced nuclear recoils.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Reporter-Spin-Assisted T 1 Relaxometry

A single-spin quantum sensor can quantitatively detect and image fluctuating electromagnetic fields via their effect on the sensor spin’s relaxation time, thus revealing important information about the target solid-state or molecular structures. However, the sensitivity and spatial resolution of spin relaxometry are often limited by the distance between the sensor and target. Here, we propose an alternative approach that leverages an auxiliary reporter spin in conjunction with a single-spin sensor, a diamond nitrogen-vacancy (N-V) center. We show that this approach can realize a 100-fold measurement sensitivity improvement for realistic working conditions and we experimentally verify the proposed method using a single shallow N-V center. Our work opens up a broad path of inquiry into a range of possible spin systems that can serve as relaxation sensors without the need for optical initialization and readout capabilities.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Bragg coherent diffraction imaging by simultaneous reconstruction of multiple diffraction peaks

Bragg coherent diffractive imaging (BCDI) is a non-invasive microscopy technique that can visualize the morphology and internal lattice deviations of crystals with nanoscale spatial resolution and picometer deformation sensitivity. While BCDI has been successfully applied in various studies of materials, it is less successful for highly-strained crystals. Specifically, it is difficult to correctly reconstruct the electron density of a highly-strained object using conventional phase retrieval algorithms. Although various algorithms have been developed to overcome this challenge, most of them require a priori knowledge that is not always available in practice. Here we report on a new phase retrieval workflow that can invert diffraction patterns from multiple Bragg peaks simultaneously. The new workflow is explored via simulated diffraction from crystals with various strain conditions. Furthermore, reconstructions from the new workflow consistently demonstrate more accurate electron density maps, in comparison with the conventional method. For highly-strained crystals, the new workflow improves the reliability and consistency of BCDI phase retrieval significantly.

36 MATERIALS SCIENCE↗

Nonequilibrium phonon tuning and mapping in few-layer graphene with infrared nanoscopy

Electron-phonon interactions are fundamentally important physical processes responsible for many key discoveries in condensed matter physics and material sciences. Herein, by exploiting the scattering-type scanning near-field optical microscope (s-SNOM) excited with a femtosecond infrared (IR) laser, we explored the strong coupling between IR phonons in few-layer graphene (FLG) with ultrahot electrons, which are heated up by the intense laser field enhanced by the s-SNOM tip. More specifically, we found that the intensity of the phonon resonance can be tuned systematically by varying the laser power that controls the electron temperature. Furthermore, the high spatial resolution of s-SNOM allows us to map the local phonon characteristics at sharp boundaries and nanostructures. Our results offer insights into the intriguing physics behind the electron-phonon interactions in nonequilibrium conditions and open a pathway for manipulating phonons with optical means.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Probing nanoparticle substrate interactions with synchrotron infrared nanospectroscopy: Coupling gold nanorod Fabry-Pérot resonances with SiO 2 and $h$-BN phonons

Spectroscopic interrogation of materials in the midinfrared with nanometer spatial resolution is inherently difficult due to the long wavelengths involved, reduced detector efficiencies, and limited availability of spectrally bright, coherent light sources. Technological advances are driving techniques that overcome these challenges, enabling material characterization in this relatively unexplored spectral regime. Synchrotron infrared nanospectroscopy (SINS) is an imaging technique that provides local sample information of nanoscale target specimens in an experimental energy window between 330 and 5000 cm -1 . Here, using SINS, we analyzed a series of individual gold nanorods patterned on a SiO 2 substrate and on a flake of hexagonal boron nitride. The SINS spectra reveal interactions between the nanorod photonic Fabry-Pérot resonances and the surface phonon polaritons of each substrate, which are characterized as avoided crossings. A coupled oscillator model of the hybrid system provides a deeper understanding of the coupling and provides a theoretical framework for future exploration.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Modeling and experimental validation of dynamical effects in Bragg coherent x-ray diffractive imaging of finite crystals

Bragg coherent diffractive imaging (BCDI) is a noninvasive microscopy technique that can visualize the shape and internal lattice deviations of crystals with nanoscale spatial resolution and picometer deformation sensitivity. Its strain imaging capability relies on Fourier transform–based iterative phase retrieval algorithms, which are mostly developed under the kinematical approximation. Such approximation prohibits the application of BCDI on larger crystals, which are commonly seen in most emerging functional materials. Understanding the dynamical effect in BCDI, as well as developing a validated method for modeling BCDI at the dynamical diffraction limit, is crucial for applying BCDI to hierarchical systems that contain micron-sized crystals and grains. Thus we report a comparative study on the impact of dynamical diffraction effects by comparing the reconstruction results from two measurements of the same crystal. Forward simulation is implemented to show subtle changes of interference fringes in the diffraction pattern due to the dynamical diffraction, and is compared directly with the experimental data.

36 MATERIALS SCIENCE↗

Jet angularities in photoproduction at the Electron-Ion Collider

We consider the one-parameter family of jet substructure observables known as angularities using the specific case of inclusive jets arising from photoproduction events at an Electron-Ion Collider (EIC). We perform numerical calculations at next-to-leading logarithmic accuracy within perturbative QCD and compare our results to PYTHIA 6 predictions. Overall, we find good agreement and conclude that jet substructure observables are feasible at the EIC despite the relatively low jet transverse momentum and particle multiplicities. We investigate the size of subleading power corrections relevant at low energies within the Monte Carlo setup. In order to establish the validity of the Monte Carlo tune, we also perform comparisons to jet shape data at HERA. We further discuss detector requirements necessary for angularity measurements at an EIC, focusing on hadron calorimeter energy and spatial resolutions. Possible applications of precision jet substructure measurements at the EIC include the tuning of Monte Carlo event generators, the extraction of nonperturbative parameters and studies of cold nuclear matter effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Nuclear two point correlation functions on a quantum computer

The calculation of dynamic response functions is expected to be an early application benefiting from rapidly developing quantum hardware resources. The ability to calculate real-time quantities of strongly correlated quantum systems is one of the most exciting applications that can easily reach beyond the capabilities of traditional classical hardware. Response functions of fermionic systems at moderate momenta and energies corresponding roughly to the Fermi energy of the system are a potential early application because the relevant operators are nearly local, and the energies can be resolved in moderately short real time, reducing the spatial resolution and gate depth required. This is particularly the case in quasielastic electron and neutrino scattering from nuclei, a topic of great interest in the nuclear and particle physics communities and directly related to experiments designed to probe neutrino properties. In this paper we use current quantum hardware and error mitigation protocols to calculate response functions for a highly simplified nuclear model through calculations of a 2-point real time correlation function for a modified Fermi-Hubbard model in two dimensions with three distinguishable nucleons on four lattice sites.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Separated reactant mix width across diffusion-dominated and hydrodynamically dominated interface mix in inertial confinement fusion implosions

Diffusion-dominated mix in inertial confinement fusion (ICF) is characterized where the majority of the mix occurs in the immediate fuel-shell interface while hydrodynamic-dominated mix pulls shell material from farther away into the central fuel. A thin (150 nm) separated reactants ICF mix platform is highly sensitive to the amount of mix from the first micron of shell-fuel interface. This fine-spatial resolution platform has revealed that material mix in moderate convergence ( CR ∼ 12 ) ICF implosions is dominated by a diffusion mechanism. This technique has now been expanded across a set of OMEGA ICF implosions, observing an increase in mix width and mix amount for cooler, slower, and more compressive implosions. Hydrodynamic simulations require a buoyancy-drag mix model to capture the increasing mix width, suggesting a transition between these two mix mechanisms. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Electronic Population Transfer via Impulsive Stimulated X-Ray Raman Scattering with Attosecond Soft-X-Ray Pulses

Free electron lasers provide a source of X-ray pulses short enough and intense enough to drive nonlinearities in molecular systems. Impulsive interactions driven by these X-ray pulses provide a way to create and probe valence electron motions with high temporal and spatial resolution. Observing these electronic motions is crucial to understand the role of electronic coherence in chemical processes. A simple nonlinear technique for probing electronic motion, impulsive stimulated X-ray Raman scattering (ISXRS), involves a single impulsive interaction to produce a coherent superposition of electronic states. In this work, we demonstrate electronic population transfer via ISXRS using broad bandwidth (5.5 eV full width at half maximum) attosecond X-ray pulses produced by the Linac Coherent Light Source (LCLS). The impulsive excitation is resonantly enhanced by the oxygen 1s → 2π* resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.

74 ATOMIC AND MOLECULAR PHYSICS↗

Accessing the Spectral Function in a Current-Carrying Device

The presence of an electrical transport current in a material is one of the simplest and most important realizations of nonequilibrium physics. The current density breaks the crystalline symmetry and can give rise to dramatic phenomena, such as sliding charge density waves, insulator-to-metal transitions, or gap openings in topologically protected states. Almost nothing is known about how a current influences the electron spectral function, which characterizes most of the solid’s electronic, optical, and chemical properties. In this work, we show that angle-resolved photoemission spectroscopy with a nanoscale light spot provides not only a wealth of information on local equilibrium properties, but also opens the possibility to access the local nonequilibrium spectral function in the presence of a transport current. Unifying spectroscopic and transport measurements in this way allows simultaneous noninvasive local measurements of the composition, structure, many-body effects, and carrier mobility in the presence of high current densities. In the particular case of our graphene-based device, we are able to correlate the presence of structural defects with locally reduced carrier lifetimes in the spectral function and a locally reduced mobility with a spatial resolution of 500 nm.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Laboratory Resolved Structure of Supercritical Perpendicular Shocks

Supermagnetosonic perpendicular flows are magnetically driven by a large radius theta-pinch experiment. Fine spatial resolution and macroscopic coverage allow the full structure of the plasma-piston coupling to be resolved in laboratory experiment for the first time. Here, a moving ambipolar potential is observed to reflect unmagnetized ions to twice the piston speed. Magnetized electrons balance the radial potential via Hall currents and generate signature quadrupolar magnetic fields. Electron heating in the reflected ion foot is adiabatic.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Observation of Fast Current Redistribution in an Imploding Plasma Column

Spectroscopic measurements of the magnetic field evolution in a Z-pinch throughout stagnation and with particularly high spatial resolution reveal a sudden current redistribution from the stagnating plasma (SP) to a low-density plasma (LDP) at larger radii, while the SP continues to implode. Based on the plasma parameters it is shown that the current is transferred to an increasing-conductance LDP outside the stagnation, a process likely to be induced by the large impedance of the SP. In conclusion, since an LDP often exists around imploding plasmas and in various pulsed-power systems, such a fast current redistribution may dramatically affect the behavior and achievable parameters in these systems.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Optical tuning of the diamond Fermi level measured by correlated scanning probe microscopy and quantum defect spectroscopy

Quantum technologies based on quantum point defects in crystals require control over the defect charge state. Here we tune the charge state of shallow nitrogen-vacancy and silicon-vacancy centers by locally oxidizing a hydrogenated surface with moderate optical excitation and simultaneous spectral monitoring. The loss of conductivity and change in work function due to oxidation are measured in atmosphere using conductive atomic force microscopy and Kelvin probe force microscopy (KPFM). We correlate these scanning probe measurements with optical spectroscopy of the nitrogen-vacancy and silicon-vacancy centers created via implantation 15–25 nm beneath the diamond surface and annealing. The observed charge state of the defects as a function of optical exposure demonstrates that laser oxidation provides a way to precisely tune the Fermi level over a range of at least 2.00 eV. We also observe a significantly larger oxidation rate for implanted surfaces compared to unimplanted surfaces under ambient conditions. Here, combined with knowledge of the electron affinity of a surface, these results suggest KPFM is a powerful, high-spatial-resolution technique to advance surface Fermi level engineering for charge stabilization of quantum defects.

36 MATERIALS SCIENCE↗

Ultrafast electron diffraction: Visualizing dynamic states of matter

Since the discovery of electron-wave duality, electron scattering instrumentation has developed into a powerful array of techniques for revealing the atomic structure of matter. Beyond detecting local lattice variations in equilibrium structures with the highest possible spatial resolution, recent research efforts have been directed toward the long-sought-after dream of visualizing the dynamic evolution of matter in real time. The atomic behavior at ultrafast timescales carries critical information on phase transition and chemical reaction dynamics, the coupling of electronic and nuclear degrees of freedom in materials and molecules, and the correlation among structure, function, and previously hidden metastable or nonequilibrium states of matter. Ultrafast electron pulses play an essential role in this scientific endeavor, and their generation has been facilitated by rapid technical advances in both ultrafast laser and particle accelerator technologies. Here this review presents a summary of the noteworthy developments in this field in the last few decades. The physics and technology of ultrafast electron beams is presented with an emphasis on the figures of merit most relevant for ultrafast electron diffraction experiments. Recent developments in the generation, manipulation, and characterization of ultrashort electron beams aimed at improving the combined spatiotemporal resolution of these measurements are discussed. The fundamentals of electron scattering from atomic matter and the theoretical frameworks for retrieving dynamic structural information from solid-state and gas-phase samples is described. Essential experimental techniques and several landmark works that have applied these approaches are also highlighted to demonstrate the widening applicability of these methods. Ultrafast electron probes with ever-improving capabilities, combined with other complementary photon-based or spectroscopic approaches, hold tremendous potential for revolutionizing our ability to observe and understand energy and matter at atomic scales.

43 PARTICLE ACCELERATORS↗

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic length scales. Our results provide direct evidence that ultrafast excitation of LaTe 3 leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

Orenstein, Gal [SLAC National Accelerator Laborato↗

Iterative X-ray spectroscopic ptychography

Spectroscopic ptychography is a powerful technique to determine the chemical composition of a sample with high spatial resolution. In spectro-ptychography, a sample is rastered through a focused X-ray beam with varying photon energy so that a series of phaseless diffraction data are recorded. Each chemical component in the material under investigation has a characteristic absorption and phase contrast as a function of photon energy. Using a dictionary formed by the set of contrast functions of each energy for each chemical component, it is possible to obtain the chemical composition of the material from high-resolution multi-spectral images. This paper presents SPA (spectroscopic ptychography with alternating direction method of multipliers), a novel algorithm to iteratively solve the spectroscopic blind ptychography problem. First, a nonlinear spectro-ptychography model based on Poisson maximum likelihood is designed, and then the proposed method is constructed on the basis of fast iterative splitting operators. SPA can be used to retrieve spectral contrast when considering either a known or an incomplete (partially known) dictionary of reference spectra. By coupling the redundancy across different spectral measurements, the proposed algorithm can achieve higher reconstruction quality when compared with standard state-of-the-art two-step methods. It is demonstrated how SPA can recover accurate chemical maps from Poisson-noised measurements, and its enhanced robustness when reconstructing reduced-redundancy ptychography data using large scanning step sizes is shown.

47 OTHER INSTRUMENTATION↗

Selected advances in small-angle scattering and applications they serve in manufacturing, energy and climate change

Innovations in small-angle X-ray and neutron scattering (SAXS and SANS) at major X-ray and neutron facilities offer new characterization tools for researching materials phenomena relevant to advanced applications. For SAXS, the new generation of diffraction-limited storage rings, incorporating multi-bend achromat concepts, dramatically decrease electron beam emittance and significantly increase X-ray brilliance over previous third-generation sources. This results in intense X-ray incident beams that are more compact in the horizontal plane, allowing significantly improved spatial resolution, better time resolution, and a new era for coherent-beam SAXS methods such as X-ray photon correlation spectroscopy. Elsewhere, X-ray free-electron laser sources provide extremely bright, fully coherent, X-ray pulses of <100 fs and can support SAXS studies of material processes where entire SAXS data sets are collected in a single pulse train. Meanwhile, SANS at both steady-state reactor and pulsed spallation neutron sources has significantly evolved. Developments in neutron optics and multiple detector carriages now enable data collection in a few minutes for materials characterization over nanometre-to-micrometre scale ranges, opening up real-time studies of multi-scale materials phenomena. SANS at pulsed neutron sources is becoming more integrated with neutron diffraction methods for simultaneous structure characterization of complex materials. In this paper, selected developments are highlighted and some recent state-of-the-art studies discussed, relevant to hard matter applications in advanced manufacturing, energy and climate change.

36 MATERIALS SCIENCE↗